Biomimetic Control over Bimetallic Nanoparticle Structure and Activity via Peptide Capping Ligand Sequence

Maichong Xie; Ryuichi Shimogawa; Yang Liu; Lihua Zhang; Alexandre C. Foucher; Prahlad K. Routh; Eric A. Stach; Anatoly I. Frenkel; Marc R. Knecht

doi:10.1021/acsnano.3c10016

Biomimetic Control over Bimetallic Nanoparticle Structure and Activity via Peptide Capping Ligand Sequence

Maichong Xie, Ryuichi Shimogawa, Yang Liu, Lihua Zhang, Alexandre C. Foucher, Prahlad K. Routh, Eric A. Stach, Anatoly I. Frenkel, Marc R. Knecht

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

The controlled design of bimetallic nanoparticles (BNPs) is a key goal in tailoring their catalytic properties. Recently, biomimetic pathways demonstrated potent control over the distribution of different metals within BNPs, but a direct understanding of the peptide effect on the compositional distribution at the interparticle and intraparticle levels remains lacking. We synthesized two sets of PtAu systems with two peptides and correlated their structure, composition, and distributions with the catalytic activity. Structural and compositional analyses were performed by a combined machine learning-assisted refinement of X-ray absorption spectra and Z-contrast measurements by scanning transmission electron microscopy. The difference in the catalytic activities between nanoparticles synthesized with different peptides was attributed to the details of interparticle distribution of Pt and Au across these markedly heterogeneous systems, comprising Pt-rich, Au-rich, and Au core/Pt shell nanoparticles. The total amount of Pt in the shells of the BNPs was proposed to be the key catalytic activity descriptor. This approach can be extended to other systems of metals and peptides to facilitate the targeted design of catalysts with the desired activity.

Original language	English
Pages (from-to)	3286-3294
Number of pages	9
Journal	ACS Nano
Volume	18
Issue number	4
DOIs	https://doi.org/10.1021/acsnano.3c10016
State	Published - Jan 30 2024
Externally published	Yes

Funding

Electron microscopy analysis of A.C.F. and E.A.S. was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award #DE-SC0012573. This research used beamline 8-ID of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used Thermo Fisher Talos 200X of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science User Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under Contract No. DE-SC0012704. This work was carried out in part at the Singh Center for Nanotechnology at the University of Pennsylvania, which is supported by the NSF National Nanotechnology Coordinated Infrastructure Program under grant NNCI-2025608. Additional support to the Nanoscale Characterization Facility at the Singh Center has been provided by the Laboratory for Research on the Structure of Matter (MRSEC) supported by the National Science Foundation (DMR-1720530). We thank E. Stavitski and D. Leshchev for assistance with the synchrotron measurements. We are grateful to Dr. Judith C. Yang for discussion of the plans for electron microscopy studies at the Center for Functional Nanomaterials at Brookhaven National Laboratory. The work was supported by the National Science Foundation under grants 2203858 (A.I.F.) and 2203862 (M.R.K.). Electron microscopy analysis of A.C.F. and E.A.S. was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award #DE-SC0012573. This research used beamline 8-ID of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used Thermo Fisher Talos 200X of the Center for Functional Nanomaterials, which is a U.S. DOE Office of Science User Facility, and the Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory under Contract No. DE-SC0012704. This work was carried out in part at the Singh Center for Nanotechnology at the University of Pennsylvania, which is supported by the NSF National Nanotechnology Coordinated Infrastructure Program under grant NNCI-2025608. Additional support to the Nanoscale Characterization Facility at the Singh Center has been provided by the Laboratory for Research on the Structure of Matter (MRSEC) supported by the National Science Foundation (DMR-1720530). We thank E. Stavitski and D. Leshchev for assistance with the synchrotron measurements. We are grateful to Dr. Judith C. Yang for discussion of the plans for electron microscopy studies at the Center for Functional Nanomaterials at Brookhaven National Laboratory. The work was supported by the National Science Foundation under grants 2203858 (A.I.F.) and 2203862 (M.R.K.).

Funders	Funder number
Center for Functional Nanomaterials at Brookhaven National Laboratory
Laboratory for Research on the Structure of Matter
National Science Foundation	DMR-1720530, 2203862, 2203858, NNCI-2025608
National Science Foundation
U.S. Department of Energy
Office of Science
Basic Energy Sciences	-SC0012573
Basic Energy Sciences
Brookhaven National Laboratory	DE-SC0012704
Brookhaven National Laboratory
Materials Research Science and Engineering Center, Harvard University

Keywords

bimetallic nanoparticles
catalysis
neural network
peptides
XAFS

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title = "Biomimetic Control over Bimetallic Nanoparticle Structure and Activity via Peptide Capping Ligand Sequence",

abstract = "The controlled design of bimetallic nanoparticles (BNPs) is a key goal in tailoring their catalytic properties. Recently, biomimetic pathways demonstrated potent control over the distribution of different metals within BNPs, but a direct understanding of the peptide effect on the compositional distribution at the interparticle and intraparticle levels remains lacking. We synthesized two sets of PtAu systems with two peptides and correlated their structure, composition, and distributions with the catalytic activity. Structural and compositional analyses were performed by a combined machine learning-assisted refinement of X-ray absorption spectra and Z-contrast measurements by scanning transmission electron microscopy. The difference in the catalytic activities between nanoparticles synthesized with different peptides was attributed to the details of interparticle distribution of Pt and Au across these markedly heterogeneous systems, comprising Pt-rich, Au-rich, and Au core/Pt shell nanoparticles. The total amount of Pt in the shells of the BNPs was proposed to be the key catalytic activity descriptor. This approach can be extended to other systems of metals and peptides to facilitate the targeted design of catalysts with the desired activity.",

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author = "Maichong Xie and Ryuichi Shimogawa and Yang Liu and Lihua Zhang and Foucher, {Alexandre C.} and Routh, {Prahlad K.} and Stach, {Eric A.} and Frenkel, {Anatoly I.} and Knecht, {Marc R.}",

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doi = "10.1021/acsnano.3c10016",

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AU - Xie, Maichong

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AU - Liu, Yang

AU - Zhang, Lihua

AU - Foucher, Alexandre C.

AU - Routh, Prahlad K.

AU - Stach, Eric A.

AU - Frenkel, Anatoly I.

AU - Knecht, Marc R.

PY - 2024/1/30

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N2 - The controlled design of bimetallic nanoparticles (BNPs) is a key goal in tailoring their catalytic properties. Recently, biomimetic pathways demonstrated potent control over the distribution of different metals within BNPs, but a direct understanding of the peptide effect on the compositional distribution at the interparticle and intraparticle levels remains lacking. We synthesized two sets of PtAu systems with two peptides and correlated their structure, composition, and distributions with the catalytic activity. Structural and compositional analyses were performed by a combined machine learning-assisted refinement of X-ray absorption spectra and Z-contrast measurements by scanning transmission electron microscopy. The difference in the catalytic activities between nanoparticles synthesized with different peptides was attributed to the details of interparticle distribution of Pt and Au across these markedly heterogeneous systems, comprising Pt-rich, Au-rich, and Au core/Pt shell nanoparticles. The total amount of Pt in the shells of the BNPs was proposed to be the key catalytic activity descriptor. This approach can be extended to other systems of metals and peptides to facilitate the targeted design of catalysts with the desired activity.

AB - The controlled design of bimetallic nanoparticles (BNPs) is a key goal in tailoring their catalytic properties. Recently, biomimetic pathways demonstrated potent control over the distribution of different metals within BNPs, but a direct understanding of the peptide effect on the compositional distribution at the interparticle and intraparticle levels remains lacking. We synthesized two sets of PtAu systems with two peptides and correlated their structure, composition, and distributions with the catalytic activity. Structural and compositional analyses were performed by a combined machine learning-assisted refinement of X-ray absorption spectra and Z-contrast measurements by scanning transmission electron microscopy. The difference in the catalytic activities between nanoparticles synthesized with different peptides was attributed to the details of interparticle distribution of Pt and Au across these markedly heterogeneous systems, comprising Pt-rich, Au-rich, and Au core/Pt shell nanoparticles. The total amount of Pt in the shells of the BNPs was proposed to be the key catalytic activity descriptor. This approach can be extended to other systems of metals and peptides to facilitate the targeted design of catalysts with the desired activity.

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Biomimetic Control over Bimetallic Nanoparticle Structure and Activity via Peptide Capping Ligand Sequence

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